RSC Advances
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2022
·Vol. 12
·期 19
·11715-11721
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IF 4.036
Baokang Zou,Yipeng Zhan,Xiuli Xie,TongTong Zhang,Runkai Qiu,Fangming Zhu
Two salalen titanium(IV) complexes ((H-salalen)TiCl2 and (F-salalen)TiCl2) containing hydrogen and fluorine respectively on the phenolate ring close to the imine were synthesized for the copolymerization of ethylene with 1-octene to prepare poly(ethylene-co-1-octene) in the presence of methylaluminoxane (MAO). The (F-salalen)TiCl2/MAO showed higher catalytic activity and better copolymer characteristics such as a higher molecular weight, narrower molecular weight distribution, and higher 1-octene incorporation than (H-salalen)TiCl2/MAO, which revealed that the electron-withdrawing conjugated effect introduced by fluorine substituents led to improvements on catalytic performance and thermal stability. The influences of copolymerization conditions including temperature, Al/Ti molar ratios and comonomer feed ratios on the copolymerization behavior of (F-salalen)TiCl2/MAO and the copolymer microstructure were investigated in detail. Under the activation of MAO, the (F-salalen)TiCl2 could produce ultrahigh molecular weight poly(ethylene-co-1-octene) with 1-octene incorporation ratios in the range of 0.9–3.1 mol% and exhibit relatively high activity. It could be inferred that long ethylene sequences in the copolymer were segregated by the isolated 1-octene units based on the 13C NMR characterization of the copolymer. Moreover, the thermal properties and crystallization of copolymers were determined by DSC and XRD and correlated to the ethylene sequence length distribution. The reactivity ratios calculated by the triad distribution in 13C NMR revealed the random comonomer distribution in the copolymer chain.
研究领域:
高分子化学
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配位聚合
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催化化学
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材料科学
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高分子物理
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高影响因子
FUEL
·
2025
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IF 7.5
Yuanyuan Cui,Gang Fu,Jiaxing Wen,Li Yang,Jiaxu Zhang,Jianmin Sun
The direct synthesis of cyclic carbonates from olefins involves a tandem process of olefin epoxidation and CO 2 cycloaddition, but designing a single catalyst with multiple active sites remains a challenge. In this work, a series of dual ligands quaternized Zr-based MOFs (Zr-Bpydc(Py + Br − )/CoTCPP-x, x = 1–5) were successfully synthesized by co-assembling 2,2′-bipyridine-5,5′-dicarboxylic acid (Bpydc) and cobalt(II) 5,10,15,20-tetrakis(4-carboxyphenyl)porphyrin (CoTCPP) with Zr 6 clusters, followed by post-synthetic quaternization to incorporate nucleophilic Br − sites. Among them, Zr-Bpydc(Py + Br − )/CoTCPP-4 exhibited the best catalytic performance under mild reaction conditions (80 °C, 1.0 MPa, 12 h), achieving styrene conversion of 94.2 % and styrene carbonate (SC) selectivity of 66.5 %, significantly outperforming most previously reported heterogeneous catalytic systems under cocatalyst-free conditions. The excellent catalytic activity was attributed to the synergistic effect among redox-active Co 2+ sites, Lewis acidic Zr 4+ and Co 2+ sites, Br − sites, and basic pyridyl sites. Importantly, the catalyst also demonstrated broad substrate applicability and good recyclability, with negligible activity loss over five consecutive cycles. Furthermore, density functional theory (DFT) calculations elucidated the energy profile and reaction pathway of the styrene oxidative carboxylation reaction, revealing the cooperative roles of multiple active sites in both epoxidation and CO 2 cycloaddition reactions. Therefore, this work proposes a strategy based on the synergy of multiple active sites for developing efficient and recyclable heterogeneous MOF catalysts for CO 2 conversion.
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APPLIED CATALYSIS A-GENERAL
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2026
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IF 4.8
Shiyu Yang,Wenqi Qin,Yanji Zhang,Jun Chai,Ronghuan Wan,Hong Lei,Yi Wei
The Pt/γ-AlOOH-IP was prepared using γ-AlOOH support by impregnation method. • The strong MSI and electron-rich Pt sites are fabricated in Pt/γ-AlOOH-IP. • Pt/γ-AlOOH-IP exhibits excellent catalytic performance in the hydrosilylation. • Electron-rich Pt sites promote the TES adsorption and Si–H bond cleavage. Hydrosilylation is a highly important method for the preparation of organosilicon compounds, in which homogeneous Pt catalysts exist poor recyclability and high production costs. Here, we prepared supported Pt-based catalyst (Pt/γ-AlOOH-IP) using γ-AlOOH support by impregnation (IP) method, in which strong metal-support interactions (MSI) and electron-rich Pt sites were fabricated. Catalytic measurements show that Pt/γ-AlOOH-IP has the best catalytic activity in the conversion of 1-octene and triethoxysilane (TES)via hydrosilylation to n-octyltriethoxysilane (OTES), the yield of OTES is 93.6% with 94.3% selectivity at 80 ℃, 2.5 h, m (Pt) /m (1-octene) = 7.5 × 10 −5 and n (TES) /n (1-octene) = 1.33, which are commensurate with homogeneous Karstedt’s catalyst. The significant catalytic performance of Pt/γ-AlOOH-IP originates from more electron transfer between Pt and γ-AlOOH. Electron-rich Pt sites promote TES chemisorption and Si–H bond dissociation, and improve catalytic activity, which are corroborated by the DFT calculations. This finding enhances the insight of MSI and offers an easy method to prepare efficient heterogeneous catalysts for industrial hydrosilylation reactions. Download: Download high-res image (166KB) Download: Download full-size image
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RSC Advances
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2026
·
IF 6.1
Baoliang Lv,Wei Zhang,Guohua Zhang,Guofu Zhang,Miao Zhang,Shoufeng Xue,Huixiang Wang
The epoxidation of long-chain α-olefins is an effective strategy for optimizing synthetic oil products and expanding their high-value-added derivatives. Tungsten trioxide (WO 3 ) is a promising catalyst for this reaction, yet pure WO 3 suffers from low specific surface area and a high density of Brønsted acid sites (B acid), resulting in poor activity and selectivity. Herein, graphene oxide (GO) was employed as a support to anchor WO 3 via an in situ growth strategy. Leveraging the strong interaction between the oxygen-containing functional groups of GO and the acidic hydroxyl groups of WO 3 , we achieved both high dispersion and effective reduction of B acid sites on WO 3 , successfully fabricating a high-performance WO 3 /GO catalyst. In the epoxidation of 1-octene, the WO 3 /GO catalyst exhibited excellent performance, specifically, its catalytic activity for producing 1,2-epoxyoctane increased from 7.9 mmol g WO 3 −1 h −1 (pure WO 3 ) to 20.3 mmol g WO 3 −1 h −1 , representing a 2.6-fold enhancement in catalytic efficiency. The catalyst also exhibited excellent performance towards other long-chain α-olefins. This study provides a simple, efficient, and dual-benefit strategy for the structural modification of WO 3 -based catalysts, offering a promising approach for designing low-acid, highly dispersed metal oxide catalysts for the efficient conversion of long-chain α-olefins. In situ anchoring of WO 3 onto GO enables high dispersion and reduced B acidity, boosting 1-octene epoxidation activity by 2.6 times.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Haijun Wu,Shenggui Ma,Dianhang Wei,Yaolin Wang,Quanwei Lv,Ziheng Jin,Xinrui Wang,Xin Tu,Xia Jiang
A strategy for plasma-coupled O v -rich catalytic hydrogen production is proposed. • The catalyst shows high activity and universality for hydrogen production. • Synergistic cascade from plasma dissociation to catalytic surface reforming. • The key mechanism of “hydrogen promotion and anti-coking” were revealed. Hydrogen production from plastics contributes to the circular economy by enabling both waste valorisation and green energy generation. Integrated pyrolysis-plasma catalytic technology offers notable advantages in improving hydrogen production, but it still faces challenges such as catalyst coking and limited understanding of the reaction mechanisms. This study proposes a water vapor plasma-coupled oxygen vacancy-rich (O v -rich) catalytic strategy to systematically investigate the improved hydrogen production from plastics over an anti-coking catalyst. The results show that the O v -rich catalyst exhibits outstanding hydrogen production activity, strong synergistic effect, and universality in the non-thermal plasma catalytic (NTP-C) reforming reaction of mixed model compounds in plastic pyrolysis oil. Crucially, its practical effectiveness was successfully validated in the NTP-C reforming of polyethylene (PE)/polypropylene (PP) pyrolysis oils. Moreover, the O v -rich catalysts significantly inhibited coking and maintained good stability for 1800 min in a multi-component mixed system. The mechanisms of hydrogen production and coking inhibition were revealed via Density Functional Theory (DFT) calculations, in situ plasma-coupled Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS), and Optical Emission Spectroscopy (OES). A synergistic reaction pathway, coupling plasma gas-phase dissociation with catalytic surface reforming, was identified as a key mechanism for enhancing hydrogen yield in plasma-catalytic systems. The study offers valuable insights for advancing plasma-assisted hydrogen production technologies. Download: Download high-res image (150KB) Download: Download full-size image
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
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IF 9.6
Li Zhou,Zetao Kang,Yifan Wang,Jiajia Gao,Kuanjun Zhang,Lei Zhao,Cheng Zhong,Dianlin Wang,Lei Xie,Jingyi Wang
Hypothesis Liquid-infused surfaces (LISs) have drawn considerable attention for their exceptional self-cleaning and antifouling properties. The interaction forces between the infusing lubricant and the substrate surface play a pivotal role in determining LIS stability and performance. However, there is a lack of directly measured intermolecular forces as quantitative experimental evidence to determine the contribution of lubricant chemistry in different environments at the molecular scale. Experiments In this study, the interaction forces of diverse functional groups representing typical infusing lubricants with polydimethylsiloxane (PDMS) and phenyltriethoxysilane (PTES) surfaces were directly measured using atomic force microscopy in air and in aqueous solution. Findings The force measurement results in air indicated that the adhesion of the functional groups was larger on PTES compared to PDMS, and the adhesion was primarily determined by van der Waals interaction. In aqueous solution, the adhesion on PTES became lower than that on PDMS across almost all the functional groups, except for the C C. This reversal could be attributed to the enhanced electrostatic repulsion between functional groups and PTES, as PTES carried more negative charges than PDMS. The large adhesion for C C on PTES measured in aqueous solution could be due to the effective π interactions between C C and the benzene ring on PTES. The force measurement results were further supported by molecular dynamics simulations, suggesting that the adhesions between lubricants and substrate surfaces were predominantly determined by the intermolecular interactions. The measured adhesion forces had a positive correlation with the lubricant retention as a higher adhesion force resulted in a lower reduction ratio of drop sliding velocity after air and water shearing. Notably, the n-octanoic acid ( COOH) exhibited the highest adhesion and the greatest resistance to shear-induced loss on PDMS both in air and under water. While 1-octene ( C C) exhibited the highest stability on PTES in an aqueous environment. This work established a molecular-level design framework for engineering robust LIS systems, offering practical guidelines for selecting lubricants suited to specific substrate surfaces. Download: Download high-res image (116KB) Download: Download full-size image
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高影响因子
RUSSIAN JOURNAL OF GENERAL CHEMISTRY
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2023
·Vol. 93
·期 1
·120-127
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IF 0.9
Huo Y. P.,Liu F.,Wu J. P.,Zhang Y. K.,Feng C. M.,Peng Y.
Abstract An imidazolyl Schiff base containing nitrogen-rich covalent organic polymer (COP) was synthesized via polycondensation reactions between bis(imidazolyl)imine-bridged bis silane and melamine under solvent thermal condition. The as-synthesized COP was then employed as a solid support for platinum catalyst. This heterogeneous catalyst was fully characterized via technics including FTIR, solid-state 13 C NMR, X-ray photoelectron spectroscopy (XPS), as well as N 2 absorption/desorption analysis, X-ray diffraction (XRD), scanning electron microscopy (SEM), and transmission electron microscopy (TEM) methods. The catalyst was efficient in mediating hydrosilylation reactions between olefins and triethoxylsilane.
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Nature Communications
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2023
·Vol. 14
·期 1
·1-11
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IF 16.6
Chen Huai,Xiong Yangyang,Li Jun,Abed Jehad,Wang Da,Pedrazo-Tardajos Adrián,Cao Yueping,Zhang Yiting,Wang Ying,Shakouri Mohsen,Xiao Qunfeng,Hu Yongfeng,Bals Sara,Sargent Edward H.,Su Cheng-Yong,Yang Zhenyu
Improving the dispersion of active sites simultaneous with the efficient harvest of photons is a key priority for photocatalysis. Crystalline silicon is abundant on Earth and has a suitable bandgap. However, silicon-based photocatalysts combined with metal elements has proved challenging due to silicon’s rigid crystal structure and high formation energy. Here we report a solid-state chemistry that produces crystalline silicon with well-dispersed Co atoms. Isolated Co sites in silicon are obtained through the in-situ formation of CoSi 2 intermediate nanodomains that function as seeds, leading to the production of Co-incorporating silicon nanocrystals at the CoSi 2 /Si epitaxial interface. As a result, cobalt-on-silicon single-atom catalysts achieve an external quantum efficiency of 10% for CO 2 -to-syngas conversion, with CO and H 2 yields of 4.7 mol g (Co) −1 and 4.4 mol g (Co) −1 , respectively. Moreover, the H 2 /CO ratio is tunable between 0.8 and 2. This photocatalyst also achieves a corresponding turnover number of 2 × 10 4 for visible-light-driven CO 2 reduction over 6 h, which is over ten times higher than previously reported single-atom photocatalysts.
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高影响因子
POLYMERS FOR ADVANCED TECHNOLOGIES
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2023
·Vol. 34
·期 6
·1979-1989
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IF 3.4
Daguang He,Xuefeng Gui,Yonglu Dong,Shudong Lin,Yuanyuan Tu,Jiwen Hu,Shi Li,Jihe Zhao
Synthetic reactions with distinctive physicochemical properties and the study of functional groups during synthesis provide an effective way to design polymers on an individual basis. The functionalization of polymethylhydrosiloxane (PMHS) has been performed via hydrosilylation of PMHS with selected alkenes with different active functional groups. In the reaction of PMHS with selected CC bond-containing olefins in solvent-free systems, the most efficient catalyst system can be selected to obtain the PMHS reagents to introduce the desired functional groups while generating only regional isomeric products. On-line real-time monitoring techniques, in situ Fourier-transform infrared (FT-IR), were utilized to determine the chemical reaction rates and reaction conversions for each chemical reaction, and to assess the merits of the reaction systems. In addition, the structures of the functionalized polymers were characterized using FT-IR spectroscopy, nuclear magnetic resonance (NMR), and gel permeation chromatography (GPC). The kinetic parameters of typical chemical reaction processes were calculated using Kissinger's equation and Ozawa's equation. The comparisons between solvent and solvent-free systems were carried out under the same conditions, and the statistics revealed that the solvent-free system was more efficient than its solvent-based counterpart. This research on the introduction of monofunctional groups into PMHS side chains might pave the way for a variety of diverse functional groups, thus allowing for the further application of PMHS and its derivatives.
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SEPARATION SCIENCE AND TECHNOLOGY
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2023
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IF 2.8
XueFeng Sun,Yueqin Song,Xiaolong Zhou
With the massive requisition of light olefins in dedicated areas of petrochemical industry, adsorption separation approaches are developed to meet the requirements. The literature studying long-chain olefins/alkanes is scarce, and the actual adsorption capacity of liquid-phase is rarely studied. In this paper, the adsorption process of Ag-10× zeolite for long-chain alkanes/olefins was systematically studied, the preparation conditions and operating conditions of the zeolite were investigated. The samples were characterized by XRD, BET and XPS. The results show that silver ions were uniformly dispersed on the surface of the zeolite. The actual adsorption capacity of the modified zeolite was determined in intermittent experiments by liquid phase concentration difference and pore volume correction. The experimental data were fitted and the results showed that the Langmuir isotherm equation was more appropriate for adsorption, indicating that the adsorbent surface was homogeneous. The quasi-secondary kinetic chemical equation was consistent with the adsorption of olefins by the modified 10× zeolite, indicating that the process was a chemisorption process. Experimental results shows that Ag-10× zeolite is an excellent adsorbent for separating long-chain olefins/alkanes mixed systems.
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高影响因子
FUEL
·
2022
·
IF 8.035
Xu Li,Jiaqi Li,Xiaohong Wang,Lijun Yang,Hong Xu,Jinxiang Dong
Despite the significant progress that has been made regarding the purification of C5–C9 linear α-olefins from the liquid products of Fischer–Tropsch synthesis, the energy-consuming separation of olefins and paraffins with the same carbon number has restricted their industrial development. Herein, we first propose a reaction-separation-utilization integrated process that combines the zirconocene/methylalumoxane-catalyzed selective dimerization of linear α-olefins to α-olefin dimers, which can then be separated from paraffins in FTS liquid products via conventional distillation and catalytically converted into branched-chain sulfonate surfactants through homogeneously organocatalytic sulfonation with sodium bisulfite. The resulting branched-chain sulfonates have been characterized by FTIR, HPLC , LC-MS, HR-MS, and NMR techniques. Their surfactant properties, including equilibrium surface tension, dynamic surface tension , foaming property, wetting ability, and emulsifying power, and detergency performance, have been thoroughly investigated. The results showed that the resulting branched-chain sulfonate surfactants exhibit superior surfactant properties and detergency performance in comparison with commercially applied linear alkylbenzene sulfonate (LAS). In view of the growing demand for anionic surfactants in the detergent and cosmetics industries , this study represents a new route for the use of α-olefins from the Fischer–Tropsch synthesis for the production of branched-chain surfactants.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2023
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IF 3.8
Chen Chen,Qiong Tang,Hong Xu,Mingxing Tang,Xuekuan Li,Lei Liu,Jinxiang Dong
Naphthenic base oil is an important lubricating base oil and very scarce in the global petroleum resources. Herein, a series of alkylated tetralin fluids similar to naphthenic base oils were produced by the alkylation of tetralin and α -olefins ( n -hexene, n -octene, n -decene) with ionic liquid Et 3 NHCl/AlCl 3 as the catalyst, where the applied raw materials are totally derived from the coal chemical industry. The product composition could be controlled by adjusting the feeding ratio of tetralin and olefin. The synthetic fluids were evaluated as lubricating base oils to reveal the structure–property correlations. Their principal physicochemical and tribological properties depend on the chain-length of α -olefins and the number of alkyl groups onto the aromatic rings. Bis-(octyl- or decyl-) alkyl tetralin exhibited good properties in terms of viscosity, thermo-oxidation stability and pour point, as well as friction-reducing and anti-wear performance, showing great potential for producing naphthenic base synthetic oils from coal-based chemicals.
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